WO2013145843A1 - Module de conversion thermoélectrique et procédé de fabrication - Google Patents

Module de conversion thermoélectrique et procédé de fabrication Download PDF

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Publication number
WO2013145843A1
WO2013145843A1 PCT/JP2013/052079 JP2013052079W WO2013145843A1 WO 2013145843 A1 WO2013145843 A1 WO 2013145843A1 JP 2013052079 W JP2013052079 W JP 2013052079W WO 2013145843 A1 WO2013145843 A1 WO 2013145843A1
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WO
WIPO (PCT)
Prior art keywords
thermoelectric conversion
conversion element
stress relaxation
electrode
layer
Prior art date
Application number
PCT/JP2013/052079
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English (en)
Japanese (ja)
Inventor
孝至 伊藤
佐藤 純一
喜男 武田
健司 田頭
Original Assignee
国立大学法人名古屋大学
日本サーモスタット株式会社
コトヒラ工業株式会社
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Application filed by 国立大学法人名古屋大学, 日本サーモスタット株式会社, コトヒラ工業株式会社 filed Critical 国立大学法人名古屋大学
Publication of WO2013145843A1 publication Critical patent/WO2013145843A1/fr

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    • HELECTRICITY
    • H10SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10NELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/80Constructional details
    • H10N10/81Structural details of the junction
    • H10N10/817Structural details of the junction the junction being non-separable, e.g. being cemented, sintered or soldered
    • HELECTRICITY
    • H10SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10NELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/10Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects
    • H10N10/17Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects characterised by the structure or configuration of the cell or thermocouple forming the device

Definitions

  • the present invention relates to a thermoelectric conversion module and a manufacturing method thereof.
  • thermoelectric conversion module used when generating power by thermoelectric conversion using exhaust heat of about 600 ° C.
  • thermoelectric conversion modules include a thermoelectric conversion element made of manganese silicide and an electrode, and a stress relaxation layer between the thermoelectric conversion element and the electrode.
  • the electrode is made of a clad material of Cu and Fe—Ni alloy (invar), and the stress relaxation layer is made of Ni foil (for example, refer to Patent Document 1).
  • the stress relaxation layer has a linear expansion coefficient of the thermoelectric conversion element and the electrode in order to prevent a bonding interface from being destroyed by a thermal stress caused by a difference in thermal expansion between the thermoelectric conversion element and the electrode.
  • Ni constituting the stress relaxation layer has a larger linear expansion coefficient than manganese silicide constituting the thermoelectric conversion element and the clad material constituting the electrode. Therefore, the conventional thermoelectric conversion module in which Ni is disposed as a stress relaxation layer between manganese silicide as a thermoelectric conversion element and the clad material as an electrode has a problem that the reliability of the joint portion is low. .
  • thermoelectric conversion element manganese silicide is used as the thermoelectric conversion element
  • Ni is used as the electrode
  • Cr— is used as the material of the stress relaxation layer disposed between the thermoelectric conversion element and the electrode.
  • a thermoelectric conversion module using a Cu alloy is conceivable.
  • the linear expansion coefficient at 500 K of the Cr—Cu alloy is 8.5 to 12.5 ⁇ 10 ⁇ 6 / K, although it varies depending on the composition.
  • the linear expansion coefficient of manganese silicide at 500K is 8.41 to 10.18 ⁇ 10 ⁇ 6 / K
  • the linear expansion coefficient of Ni at 500K is 15.3 ⁇ 10 ⁇ 6 / K. . That is, depending on the composition of the Cr—Cu alloy, the coefficient of linear expansion can be made larger than that of manganese silicide constituting the thermoelectric conversion element and smaller than Ni constituting the electrode.
  • thermoelectric conversion module including the Cr—Cu alloy between the thermoelectric conversion element and the electrode
  • the Cr—Cu alloy can effectively act as a stress relaxation layer. It is considered that the electrode can be satisfactorily bonded.
  • thermoelectric conversion module Cr and Cu constituting the stress relaxation layer diffuse into the thermoelectric conversion element due to heat during manufacturing and use, and react with silicon in manganese silicide to react with chromium silicide, etc. Form.
  • the thermoelectric conversion module has a disadvantage that the thermoelectric conversion characteristics of the thermoelectric conversion element change and the output becomes unstable.
  • An object of the present invention is to provide a thermoelectric conversion module that can eliminate such inconvenience, obtain good bonding properties, and maintain the performance of a thermoelectric conversion element, and a method for manufacturing the same.
  • thermoelectric conversion element made of manganese silicide, an electrode, and a stress relaxation layer made of a Cr—Cu alloy disposed between the thermoelectric conversion element and the electrode.
  • a thermoelectric conversion module comprising: a diffusion prevention for preventing diffusion of Cr and Cu constituting the stress relaxation layer into the thermoelectric conversion element, which is made of Ni between the thermoelectric conversion element and the stress relaxation layer It is characterized by comprising a layer.
  • thermoelectric conversion module of the present invention Cr and Cu constituting the stress relaxation layer diffuse to the thermoelectric conversion element side due to heat during manufacture and use.
  • the diffusion prevention layer is disposed between the stress relaxation layer and the thermoelectric conversion element, the diffusion of Cr and the diffusion of Cu remain inside the diffusion prevention layer, and the thermoelectric It does not reach the inside of the conversion element. Therefore, the thermoelectric conversion module of the present invention can prevent the performance degradation of the thermoelectric conversion element due to the diffusion of Cr and the diffusion of Cu.
  • thermoelectric conversion module of the present invention although Ni constituting the diffusion preventing layer diffuses inside the thermoelectric conversion element due to heat during manufacture and use, the diffused Ni is the thermoelectric conversion of the thermoelectric conversion element. Since the characteristics are not impaired, the performance of the thermoelectric conversion element can be maintained.
  • Ni which comprises the said diffusion prevention layer diffuses in the inside of the said thermoelectric conversion element, This diffusion prevention layer and this thermoelectric conversion element can be joined favorably.
  • thermoelectric conversion module of the present invention good bondability can be obtained and the performance of the thermoelectric conversion element can be maintained.
  • thermoelectric conversion module of the present invention it is preferable to use one kind of metal selected from the group consisting of Ni, Mo, and W as the electrode.
  • Ni, Mo, and W are all advantageous as an electrode of a thermoelectric conversion module because they have low electrical resistivity and high thermal conductivity.
  • the manufacturing method of the thermoelectric conversion module of the present invention includes superimposing the diffusion prevention layer on the stress relaxation layer and heating the thermoelectric conversion element on the diffusion prevention layer, thereby heating the stress relaxation layer and the stress relaxation layer. Bonding the diffusion prevention layer and the thermoelectric conversion element to form a thermoelectric conversion element structure; and on the surface of the thermoelectric conversion element structure opposite to the diffusion prevention layer of the stress relaxation layer, And a step of joining the electrodes.
  • the diffusion prevention layer is overlaid on the stress relaxation layer, and the thermoelectric conversion element is overlaid on the diffusion prevention layer and heated. Thereby, the stress relaxation layer, the diffusion preventing layer, and the thermoelectric conversion element are bonded to form the thermoelectric conversion element structure.
  • thermoelectric conversion module can be obtained by bonding the electrode to the surface of the thermoelectric conversion element structure opposite to the diffusion preventing layer of the stress relaxation layer.
  • the step of joining the stress relaxation layer and the diffusion prevention layer to form a joined body, and the stress relaxation layer of the diffusion prevention layer of the joined body include: A step of joining the joined body and the thermoelectric conversion element to form a thermoelectric conversion element structure by superimposing and heating the thermoelectric conversion element on the opposite surface, and the thermoelectric conversion element structure A step of bonding the electrode to a surface of the stress relaxation layer opposite to the diffusion preventing layer.
  • the stress relaxation layer and the diffusion prevention layer are joined to form a joined body.
  • thermoelectric conversion element is overlaid and heated on the surface of the joined body opposite to the stress relaxation layer of the diffusion preventing layer. Thereby, the said joined body and the said thermoelectric conversion element are joined, and a thermoelectric conversion element structure is formed.
  • thermoelectric conversion module can be obtained by bonding the electrode to the surface of the thermoelectric conversion element structure opposite to the diffusion preventing layer of the stress relaxation layer.
  • FIG. 1 is a diagram illustrating a configuration of a thermoelectric conversion module according to the present embodiment.
  • 2A is a diagram illustrating a method for manufacturing a thermoelectric conversion module according to the present embodiment
  • FIG. 2B is a diagram illustrating a method for manufacturing the thermoelectric conversion module according to the present embodiment
  • FIG. 2C is a diagram illustrating the method according to the present embodiment.
  • FIG. 3A is a diagram showing a method for manufacturing the thermoelectric conversion module of the present embodiment
  • FIG. 3B is a diagram showing a method for manufacturing the thermoelectric conversion module of the present embodiment
  • FIG. 3C is a diagram of the present embodiment.
  • thermoelectric conversion module 1 of this embodiment shown in FIG. 1 is used when generating power by thermoelectric conversion using exhaust heat of about 600 ° C.
  • the thermoelectric conversion module 1 includes a pair of electrodes 3 formed on an insulating substrate 2, a pair of stress relaxation layers 4 made of a Cr—Cu alloy bonded to each electrode 3, and bonded to each stress relaxation layer 4.
  • a pair of diffusion prevention layers 5 made of Ni and a thermoelectric conversion element 6 made of manganese silicide sandwiched and joined by the pair of diffusion prevention layers 5 are provided.
  • the electrode 3 one kind of metal selected from the group consisting of Ni, Mo and W can be used. All of Ni, Mo, and W are advantageous as the electrode 3 of the thermoelectric conversion module 1 because they have low electrical resistivity and high thermal conductivity. In this embodiment, Ni is used.
  • the Cr—Cu alloy constituting the stress relaxation layer 4 has a mass ratio of Cr to Cu of 45:55 to 55:45, and is composed of a Cu matrix and a flat Cr phase.
  • the Cr—Cu alloy has a linear expansion coefficient at 500K of 9.5 to 12.5 ⁇ 10 ⁇ 6 / K when the mass ratio of Cr and Cu is 45:55, and the mass ratio of Cr and Cu is It is 9 to 12 ⁇ 10 ⁇ 6 / K when 50:50, and 8.5 to 11.5 ⁇ 10 ⁇ 6 / K when the mass ratio of Cr and Cu is 55:45.
  • the diffusion prevention layer 5 has a sufficient thickness of, for example, about 5 ⁇ m or more in order to prevent diffusion of Cr and Cu from the stress relaxation layer 4 to the thermoelectric conversion element 6.
  • thermoelectric conversion module 1 of the present embodiment Cr and Cu constituting the stress relaxation layer 4 diffuse into the diffusion prevention layer 5 due to heat during manufacture and use, and Ni constituting the diffusion prevention layer 5 Diffuses into the thermoelectric conversion element 6.
  • the stress relaxation layer 4, the diffusion prevention layer 5, and the thermoelectric conversion element 6 can be favorably bonded.
  • the diffusion prevention layer 5 made of Ni is disposed between the stress relaxation layer 4 and the thermoelectric conversion element 6, the Cr and Cu are diffused by heat during manufacture and use. Reaching the inside of the thermoelectric conversion element 6 can be prevented. Thereby, the performance fall of the thermoelectric conversion element 6 by the spreading
  • thermoelectric conversion characteristics of the thermoelectric conversion element 6 are not impaired by diffusion of Ni, the performance of the thermoelectric conversion element 6 can be maintained.
  • thermoelectric conversion module 1 of the present embodiment good bondability can be obtained, and the performance of the thermoelectric conversion element 6 can be maintained.
  • thermoelectric conversion module 1 of the present embodiment Next, a first manufacturing method of the thermoelectric conversion module 1 of the present embodiment will be described with reference to FIG.
  • a porous body made of Cr is obtained by firing Cr powder.
  • a metal plate made of a Cr—Cu alloy in which the mass ratio of Cr to Cu is in the range of 45:55 to 55:45 is obtained. obtain.
  • the obtained metal plate is cold-rolled to form, for example, a Cr—Cu alloy foil having a thickness of 250 ⁇ m.
  • the Cr—Cu alloy foil is subjected to softening aging heat treatment.
  • Cr—Cu alloy foils 4a and 4b having a thickness of 250 ⁇ m and made of a Cr—Cu alloy having a mass ratio of Cr and Cu in the range of 45:55 to 55:45 can be obtained.
  • SPS Spark ⁇ ⁇ Plasma Sintering
  • the discharge plasma sintering can be performed, for example, by applying a direct current pulse under pressure to the mixed powder charged in a die in a vacuum atmosphere.
  • one Ni foil 5a is overlaid on one obtained Cr—Cu alloy foil 4a, and the obtained thermoelectric conversion element is formed on the Ni foil 5a. 6 is overlapped. Further, the other Ni foil 5b is superposed on the thermoelectric conversion element 6, and the other Cr—Cu alloy foil 4b obtained is superposed on the Ni foil 5b.
  • said Ni foil 5a, 5b what has thickness of about 5 micrometers or more can be used, for example.
  • the Cr—Cu alloy foil 4a, the Ni foil 5a, the thermoelectric conversion element 6, the Ni foil 5b, and the Cr—Cu alloy foil 4b that are integrally stacked are heated by discharge plasma sintering.
  • a Cr—Cu alloy foil 4a, a Ni foil 5a, a thermoelectric conversion element 6, a Ni foil 5b, and a Cr—Cu alloy foil 4b are stacked under a direct current under pressure. Can be performed by applying a pulse.
  • thermoelectric conversion element structure 7 formed by bonding the stress relaxation layer 4 made of a Cu alloy can be obtained.
  • thermoelectric conversion element structure 7 is cut into a desired dimension by a wire saw, a dicing saw or the like.
  • an electrode 3 made of Ni is formed on the insulating substrate 2 by brazing or metallizing the Ni layer on the insulating substrate 2.
  • thermoelectric conversion module 1 shown in FIG. 1 can be obtained.
  • the Cr—Cu alloy foil 4 a, the Ni foil 5 a, the thermoelectric conversion element 6, the Ni foil 5 b, and the Cr—Cu alloy foil 4 b are integrally laminated by discharge plasma sintering.
  • the thermoelectric conversion element structure 7 is formed by heating by.
  • the stress relaxation layer 4 made of a Cr—Cu alloy, the diffusion preventing layer 5 made of Ni, and the thermoelectric conversion element 6 can be satisfactorily bonded.
  • the mixed powder of Mn and Si is heated by discharge plasma sintering to synthesize a manganese silicide sintered body, and the thermoelectric conversion element 6 is formed. Then, hot pressing may be performed.
  • the discharge plasma sintering is performed by integrally stacking the Cr—Cu alloy foil 4a, the Ni foil 5a, the thermoelectric conversion element 6, the Ni foil 5b, and the Cr—Cu alloy foil 4b.
  • the thermoelectric conversion element structure 7 is formed by heating, the sintering may be performed under high temperature and high pressure using an inert gas such as argon or nitrogen as a pressure medium instead of the discharge plasma sintering.
  • the Cr—Cu alloy foil 4 a, the Ni foil 5 a, the thermoelectric conversion element 6, the Ni foil 5 b, and the Cr—Cu alloy foil 4 b are integrally stacked to heat the thermoelectric element.
  • the conversion element structure 7 may be as follows. First, an intermediate structure is formed by heating the integrally laminated Cr—Cu alloy foil 4a, Ni foil 5a, and thermoelectric conversion element 6. Next, the Ni foil 5b and the Cr—Cu alloy foil 4b are integrally overlapped and heated on the surface opposite to the Ni foil 5a of the thermoelectric conversion element 6 of the obtained intermediate structure, The thermoelectric conversion element structure 7 can be obtained.
  • the thermoelectric conversion element structure 7 includes one Cr—Cu alloy foil 4a, one Ni foil 5a, the thermoelectric conversion element 6, the other Ni foil 5b, and the other Cr—Cu alloy.
  • the foil 4b is superposed, heated, joined, and then cut to form the desired dimensions, but the following may be used.
  • a manganese silicide sintered body is manufactured by charging the mixed powder into a die having a desired dimension and heating the mixed powder.
  • one Cr—Cu alloy foil 4a and one Ni foil 5a cut to the desired dimensions, the thermoelectric conversion element 6 made of the sintered body formed to the desired dimensions, and the desired dimensions are cut.
  • the thermoelectric conversion element structure 7 having a desired dimension can be obtained.
  • thermoelectric conversion module 1 including a plurality of thermoelectric conversion elements 6 arranged in parallel or in series can be formed.
  • thermoelectric conversion module 1 of the present embodiment Next, the second manufacturing method of the thermoelectric conversion module 1 of the present embodiment will be described with reference to FIG.
  • a Cr—Cu alloy foil having a thickness of 250 ⁇ m is formed of a Cr—Cu alloy in which the mass ratio of Cr and Cu is in the range of 45:55 to 55:45. To do.
  • a Ni foil is superposed on the obtained Cr—Cu alloy foil, and then heated by spark plasma sintering.
  • the discharge plasma sintering can be performed, for example, by applying a direct current pulse under pressure on a laminate of the Cr—Cu alloy foil and the Ni foil in a vacuum atmosphere.
  • thermoelectric conversion element 6 is superimposed on the surface of the obtained bonded body 8 opposite to the stress relaxation layer 4 of the diffusion preventing layer 5.
  • the other joined body 8 is superposed on the surface of the thermoelectric conversion element 6 opposite to the joined body 8 so that the surface of the diffusion preventing layer 5 opposite to the stress relaxation layer 4 is directed to discharge plasma.
  • Heat by sintering The spark plasma sintering is performed by subjecting the Cr—Cu alloy foil 4a, the Ni foil 5a, the thermoelectric conversion element 6, the Ni foil 5b, and the Cr—Cu alloy foil 4b to the one in the first manufacturing method. Can be performed under exactly the same conditions.
  • thermoelectric conversion element structure 7 is made of a stress relaxation layer 4 made of a Cr—Cu alloy, a diffusion prevention layer 5 made of Ni, a thermoelectric conversion element 6, a diffusion prevention layer 5 made of Ni, and a Cr—Cu alloy. It is formed by joining the stress relaxation layer 4.
  • thermoelectric conversion element structure 7 is cut into a desired dimension in exactly the same manner as in the first manufacturing method.
  • an electrode 3 made of Ni is formed on the insulating substrate 2 in exactly the same manner as in the first manufacturing method.
  • thermoelectric conversion module 1 shown in FIG. 1 can be obtained.
  • thermoelectric conversion element structure 7 is formed by heating the superposed laminate 8 on the other joined body 8 by discharge plasma sintering.
  • thermoelectric conversion element structure 7 is formed by heating the one bonded body 8, the thermoelectric conversion element 6, and the other bonded body 8 that are integrally overlapped. It may be as follows. First, one joined body 8 and the thermoelectric conversion element 6 are heated to form an intermediate structure. Next, the thermoelectric conversion element structure 7 is obtained by superimposing and heating the other bonded body 8 on the surface opposite to the one bonded body 8 of the thermoelectric conversion element 6 of the obtained intermediate structure. be able to.
  • thermoelectric conversion element structure 7 is formed by superposing one joined body 8, the thermoelectric conversion element 6 and the other joined body 8, heating and joining them, and then cutting them. Although it is formed in a desired dimension, each joined body 8 and thermoelectric conversion element 6 formed in a desired dimension may be superposed and heated to be joined.
  • thermoelectric conversion module 1 including a plurality of thermoelectric conversion elements 6 arranged in parallel or in series can be formed.

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Abstract

Module de conversion thermoélectrique grâce auquel de bonnes propriétés de liaison peuvent être obtenues et les performances de l'élément de conversion thermoélectrique peuvent être conservées. L'invention concerne également un procédé de fabrication du module de conversion thermoélectrique. Un module de conversion thermoélectrique (1) pourvu d'un élément de conversion thermoélectrique (6) comprenant du siliciure de manganèse, une électrode (3), et une couche de relaxation des contraintes (4) comprenant un alliage Cr-Cu et installé entre l'élément de conversion thermoélectrique (6) et l'électrode (3) est prévu, entre l'élément de conversion thermoélectrique (6) et la couche de relaxation des contraintes (4), avec une couche de prévention de diffusion (5), comprenant du Ni, pour empêcher la diffusion de Cr et Cu constituant la couche de relaxation des contraintes (4) dans l'élément de conversion thermoélectrique (6). L'électrode (3) est un type de métal choisi dans le groupe constitué de Ni, Mo et W.
PCT/JP2013/052079 2012-03-26 2013-01-30 Module de conversion thermoélectrique et procédé de fabrication WO2013145843A1 (fr)

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JP2012-070091 2012-03-26
JP2012070091A JP2013201382A (ja) 2012-03-26 2012-03-26 熱電変換モジュール及びその製造方法

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20180059830A (ko) 2015-09-28 2018-06-05 미쓰비시 마테리알 가부시키가이샤 열전 변환 모듈 및 열전 변환 장치
WO2019170826A1 (fr) 2018-03-07 2019-09-12 Rgs Development B.V. Dispositif de conversion thermoélectrique et son procédé de fabrication
JP2020096076A (ja) * 2018-12-12 2020-06-18 昭和電線ケーブルシステム株式会社 熱電変換モジュール、および、その製造方法

Families Citing this family (5)

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Publication number Priority date Publication date Assignee Title
NO341705B1 (en) 2016-02-22 2018-01-02 Tegma As Thermoelectric half-cell and method of production
JP7242999B2 (ja) * 2018-03-16 2023-03-22 三菱マテリアル株式会社 熱電変換素子
WO2019177147A1 (fr) * 2018-03-16 2019-09-19 三菱マテリアル株式会社 Élément de conversion thermoélectrique
JP6733706B2 (ja) * 2018-06-12 2020-08-05 ヤマハ株式会社 熱電変換モジュール
JP7248091B2 (ja) * 2021-02-03 2023-03-29 三菱マテリアル株式会社 熱電変換モジュール、および、熱電変換モジュールの製造方法

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JP2003309294A (ja) * 2002-02-12 2003-10-31 Komatsu Ltd 熱電モジュール
JP2010109054A (ja) * 2008-10-29 2010-05-13 Kyocera Corp 熱電変換モジュールならびに冷却装置、発電装置および温度調節装置
JP2011249492A (ja) * 2010-05-26 2011-12-08 Furukawa Co Ltd 熱電変換モジュール

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JP2003309294A (ja) * 2002-02-12 2003-10-31 Komatsu Ltd 熱電モジュール
JP2010109054A (ja) * 2008-10-29 2010-05-13 Kyocera Corp 熱電変換モジュールならびに冷却装置、発電装置および温度調節装置
JP2011249492A (ja) * 2010-05-26 2011-12-08 Furukawa Co Ltd 熱電変換モジュール

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20180059830A (ko) 2015-09-28 2018-06-05 미쓰비시 마테리알 가부시키가이샤 열전 변환 모듈 및 열전 변환 장치
US10573798B2 (en) 2015-09-28 2020-02-25 Mitsubishi Materials Corporation Thermoelectric conversion module and thermoelectric conversion device
WO2019170826A1 (fr) 2018-03-07 2019-09-12 Rgs Development B.V. Dispositif de conversion thermoélectrique et son procédé de fabrication
JP2020096076A (ja) * 2018-12-12 2020-06-18 昭和電線ケーブルシステム株式会社 熱電変換モジュール、および、その製造方法

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